EP1652258A2 - Unite membrane-electrodes pour electrolyse de l'eau - Google Patents

Unite membrane-electrodes pour electrolyse de l'eau

Info

Publication number
EP1652258A2
EP1652258A2 EP04741011A EP04741011A EP1652258A2 EP 1652258 A2 EP1652258 A2 EP 1652258A2 EP 04741011 A EP04741011 A EP 04741011A EP 04741011 A EP04741011 A EP 04741011A EP 1652258 A2 EP1652258 A2 EP 1652258A2
Authority
EP
European Patent Office
Prior art keywords
membrane
gas distributor
ion
conducting
catalyst layer
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
Application number
EP04741011A
Other languages
German (de)
English (en)
Other versions
EP1652258B1 (fr
Inventor
Ralf Zuber
Klaus Schaack
Sandra Wittpahl
Holger Dziallas
Peter Seipel
Pia Braun
Lutz Rohland
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Umicore AG and Co KG
Original Assignee
Umicore AG and Co KG
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Priority claimed from US10/699,158 external-priority patent/US20050014056A1/en
Application filed by Umicore AG and Co KG filed Critical Umicore AG and Co KG
Publication of EP1652258A2 publication Critical patent/EP1652258A2/fr
Application granted granted Critical
Publication of EP1652258B1 publication Critical patent/EP1652258B1/fr
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

Links

Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/1004—Fuel cells with solid electrolytes characterised by membrane-electrode assemblies [MEA]
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
    • C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
    • C25B9/23—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms comprising ion-exchange membranes in or on which electrode material is embedded
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8605—Porous electrodes
    • H01M4/8626—Porous electrodes characterised by the form
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8878—Treatment steps after deposition of the catalytic active composition or after shaping of the electrode being free-standing body
    • H01M4/8896—Pressing, rolling, calendering
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0247—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the form
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • the present invention describes a membrane electrode assembly ("MEE") for use in PEM water electrolysers.
  • the membrane electrode unit can also be used for regenerative fuel cells (RBC) or for oxygen-generating electrodes in various other areas of electrolysis.
  • RBC regenerative fuel cells
  • a method for producing the membrane electrode unit is described.
  • Electrolysis of water is the most practical method to produce hydrogen using renewable energy sources.
  • the investment and production costs for electrolysers determine the overall economy of the system and therefore decide whether this will be a viable process for the production of hydrogen.
  • the cost of producing hydrogen through the electrolysis of water is largely affected by the consumption of electrical energy, which can amount to about 70% of the total cost of producing hydrogen.
  • PEM electrolyte membrane Able to operate at much higher current densities and with a lower specific energy consumption compared to conventional alkali-containing electrolysers, so that they are characterized by the advantage of higher plant utilization and lower production costs Improving water electrolysis processes using PEM electrolysers and, in particular, providing improved membrane electrode assemblies (MEEs) for PEM electrolysers
  • PEM electrolysers are constructed similarly to a PEM fuel cell, but they work in different ways.
  • An MEE for a PEM water electrolyzer (hereinafter also referred to as “electrolysis MEE”) generally contains a polymer electrolyte membrane (for example Nafion® from DuPont), which is sandwiched between two electrodes and two porous current collectors (or gas distributor substrates). , which are mounted on both sides of the electrodes.
  • a polymer electrolyte membrane for example Nafion® from DuPont
  • the electrolysis MEE has a differential pressure between Anode and cathode is exposed, which is about 5 to 10 times higher than when operating a conventional PEM fuel cell.
  • Thicker membrane materials are therefore preferably used (up to 200 ⁇ m thick).
  • new MEE construction concepts are necessary, as described in the present application. (c) Since oxygen is produced in addition to hydrogen during the electrolysis process, there is a latent risk of a detonating gas explosion in the event of a leak. The reactants must be strictly separated from one another in order to avoid such effects. There are therefore increased demands on the gas tightness of the electrolysis MEEs.
  • iridium is known for its unique electrocatalytic properties related to chlorine and oxygen release processes. Therefore, iridium is the preferred material for the oxygen development reaction (OER) on the anode side, either in the form of the pure metal (as "Mohr") or as an oxide, possibly in a mixture with other oxides.
  • OER oxygen development reaction
  • Suitable anode catalysts for electrolysis MEEs are described, for example, in the applicant's German patent application P 1 0350 563.6. Of all the precious metals, platinum is the most active catalyst for the reaction to release the hydrogen (HER) at the cathode and is frequently used as a cathode catalyst in electrolysis MEEs. For these reasons, conventional MEEs, such as those used for PEM fuel cells, cannot be used for PEM electrolysers.
  • catalyst inks which comprise catalyst powder, solvent and optionally polymer electrolyte material (ie a dissolved ionomer) are produced and either applied directly to the ionomer membrane or first applied to the gas distributor substrate and then connected to the membrane (see, for example, the patents US 5,861,222; US 6,309,772 and US 6,500,217 by the applicant). Problems with the registration accuracy and dimensional stability of the motifs occur in particular when coating the ionomer membranes on both sides.
  • the electrolysis MEE should be able to be manufactured in a simple, inexpensive process without high membrane consumption.
  • the process should have low error tolerances and high register accuracy and should therefore be suitable for mass production. This object is achieved by the provision of an invention
  • the membrane-electrode unit according to the invention for the electrolysis of water is shown in FIG. 1, the individual components being shown schematically before assembly.
  • the MEE contains an ion-conducting membrane with front and back (1), a first catalyst layer on the front (cathode side) for hydrogen evolution (2), a first gas distributor substrate on the front (4), a second catalyst layer on the back (anode side ) for anodic oxygen generation (3), and a second gas distributor substrate on the back (5).
  • the first gas distribution substrate (4) has a smaller area expansion than the ion-conducting membrane (1) and the second gas distribution substrate (5) has essentially the same area extension as the ion-conducting membrane (1).
  • FIG. 2 shows the electrolysis MEA according to the invention in the assembled state (5-layer structure).
  • the sealing material in the edge area (7) encloses the MEE in a gas-tight manner and, due to the free membrane surface (6), has improved adhesive strength and gas-tightness. Additional consumption of membrane material for sealing purposes in the edge area is avoided.
  • the gas distributor substrate (5) can be omitted.
  • an MEE which contains an ion-conducting membrane with front and rear sides (1), a first catalyst layer on the front side (2), a first gas distributor substrate on the front side (4) and a second catalyst layer on the rear side (3) ,
  • This 4-layer MEE is surrounded by a sealing material (7) in the edge area. There is no additional consumption of membrane material in the edge area.
  • the MEE according to the invention contains a free membrane edge (6) that is not supported by a gas distributor substrate.
  • the edge area ie the distance from the outer edge of the membrane (1) to the outer edge of the smaller gas distributor substrates (4) on the cathode side, is small and has a width of at least 0.5 mm all around, preferably a width, in the assembled membrane-electrode unit of at least 1 mm. For cost reasons, the edge width should be limited to a maximum of 5 mm all around.
  • the electrolysis MEA according to the invention has a called "semi-extensive design" with regard to the two gas distributor substrates (4) and (5).
  • the manufacturing process for the electrolysis MEEs consists of a combined process of membrane coating (“CCM process”) and gas distributor substrate coating (“CCB process”), both substrates being coated on one side only with catalyst. This avoids the problems of register accuracy and dimensional stability with multi-sided printing. However, one side of the substrate can be coated several times to achieve a higher catalyst loading.
  • CCM process membrane coating
  • CB process gas distributor substrate coating
  • the noble metal catalysts are processed into inks or pastes, using suitable solvents and possibly with the addition of ionomer materials.
  • the catalyst for the cathode is applied to a gas distributor substrate, the catalyst for the A-node directly onto the ionomer membrane.
  • the typical catalyst loading of the anode is in the range from 0.5 to 4 mg noble metal / cm 2 , preferably catalysts containing tr or Ir oxide are used here.
  • Standard platinum catalysts eg Pt / C or Pt-Mohr
  • the cathode loads are in the range from 0.2 to 1 mg Pt / cm 2 .
  • a drying process is generally performed thereafter to remove the solvents from the catalyst inks.
  • the carbon-based gas distribution substrates for the cathode can consist of porous, electrically conductive materials such as, for example, graphitized or carbonized carbon fiber papers, carbon fiber nonwovens, carbon fiber fabrics and / or the like.
  • the non-carbon-based gas diffusion layer on the anode side can contain a metal mesh, metal mesh, metal fleece, metal staple fiber, metal multi-filament and / or another porous metallic structure.
  • titanium sintered plates type SIKA-T10®, GKN, Radevormwald
  • the ion-conducting membrane generally consists of proton-conducting polymer materials.
  • a tetrafluoroethylene-fluoro-vinyl ether copolymer with sulfonic acid groups is preferably used.
  • This material is sold by DuPont under the trade name Nafion ® .
  • fluorine-free, ionomer materials such as doped sulfonated polyether ketones or doped sulfonated or sulfinated aryl ketones and doped polybenzimidazoles, can also be used.
  • Composite membranes, reinforced membranes, ceramic membrane Ranes and multilayer membrane materials can also be used.
  • organic polymers can be used which are inert under the working conditions of water electrolysis and do not secrete any interfering substances.
  • the polymers must be able to enclose the gas distribution substrates in a gas-tight manner. Other important requirements for such polymers are good adhesiveness and good wetting properties to the free surface of the ion-conducting membrane.
  • Suitable materials include thermoplastic polymers such as polyethylene, polypropylene, PTFE, PVDF, polyamide, polyimide, polyurethane or polyester; on the other hand also thermosetting polymers such as epoxy resins or cyanoacrylates.
  • elastomers such as silicone rubber, EPDM, fluoroelastomers, perfluoroelastomers, chloroprene elastomers and fluorosilicone elastomers.
  • pre-cut foils for sealing or for edging the membrane electrode unit according to the invention
  • it can be inserted into a press between two corresponding pre-cut frames made of thermoplastic material.
  • the frames are cut in such a way that their inner foam encompasses the shape of the respective active surface as precisely as possible.
  • the polymeric film material is then melted using heat and pressure. It then encompasses the outer area of the semi-extensive gas diffusion layer as well as the free surface of the membrane.
  • the gas distribution substrates (4, 5) of the electrolysis MEA according to the invention can still be impregnated gas-tight in their peripheral area with polymer material.
  • frames made of thermoplastic polymer can be cut so that their inner cutout encompasses the shape of the active hache as precisely as possible.
  • the overall height of the frames is slightly larger than the height of the cavity in the mold.
  • the polymeric material is then melted using heat and pressure.
  • the height of the frame is reduced to that of the mold by the pressing pressure, as a result of which the polymer impregnates the peripheral region of the gas distributor substrate continuous to the membrane and cohesively encloses the exposed surface of the membrane and the gas diffusion layer (s).
  • the sealing material should penetrate the edge area of the MEE to a depth of at least 1 mm, preferably at least 2 mm. This gives very good results with regard to pressure stability.
  • the same result can be achieved by using polymeric sealing materials in liquid form.
  • the penetration area of the sealing material can be controlled by its viscosity and wetting properties.
  • curing of the polymeric sealing material can take place through contact with atmospheric moisture and / or at elevated temperature.
  • the invention is illustrated by the following examples without, however, being restricted thereto.
  • the gas distribution substrate (5) is made from a membrane coated on one side.
  • the corresponding membrane Nafion® N 117, Du Pont
  • An iridium oxide powder BET surface area approx. 30 m 2 / g, Umicore
  • the catalyst ink has the following composition:
  • the catalyst loading is 2 mg Ir / cm 2 .
  • the catalyst-coated membrane is then dried at 90 ° C.
  • the required format (punch size 5 x 5 cm; active area 25 cm 2 ) is then punched out in such a way that the membrane is completely coated with catalyst on one side.
  • a second step based on a gas distributor substrate
  • the gas distribution substrate is coated by means of a screen printing process with a paste which has the following composition: 18.5 g of Pt / C catalyst (60% by weight of platinum on carbon black; Umicore) 55.0 g of Nafion® (10% by weight in Water, DuPont) 26.5 g propylene glycol
  • the catalyst loading is 0.57 mg Pt / cm 2 .
  • the gas distributor substrate is then dried at 110 ° C.
  • a format (punch size 4.7 x 4.7 cm, active area 22.1 cm 2 ) is punched out of the catalyst-coated substrate on one side, so that the electrode obtained is coated over the entire area with catalyst.
  • a 4-layer MEE is produced by laminating the coated membrane and the coated gas distributor substrate with one another in such a way that the catalyst layer of the gas distributor substrate is bonded to the as yet uncoated side of the membrane. This results in a 1.5 mm wide edge of free membrane around the periphery of the arrangement.
  • the lamination takes place at 150 ° C with a pressure of 150 N / cm 2 .
  • the MEE described is provided with a frame made of sealing material, which enables installation in the electrolyzer and good sealing.
  • a press tool is used which has a cutout measuring 120 x 120 x 0.5 mm 3 .
  • the 4-layer MEA is inserted into this recess together with two frames made of Vestamelt® (polyamide; Degussa, Duesseldorf).
  • the frames each have an external dimension of 11 x 11 cm and a height of 0.29 mm.
  • a frame has an internal dimension of 4.7 x 4.7 cm, the other one of 5 x 5 cm.
  • the loaded pressing tool is placed in a hot press and a heating surface temperature of 170 ° C. is applied for 60 seconds.
  • a pressing force of at least 10 tons is achieved.
  • the electrolysis MEE is removed and punched to its final dimensions.
  • Two MEEs produced according to this process were joined on the anode side with a titanium sintering plate (SIKA-T10®, thickness 2 mm; GKN, Radevormwald) measuring 4.9 x 4.9 cm and installed in an electrolytic cell.
  • a current / voltage curve is recorded without pressure at a cell temperature of 80 ° C. The following values are obtained for the electrolysis voltage at different current densities:
  • a press tool is again used, in the recess of which the 5-layer MEE is inserted together with two Vestamelt® frames (from Degussa, Duesseldorf).
  • the frames each have an outer dimension of 11 x 11 cm.
  • a frame has an internal dimension of 4.7 x 4.7 cm and a height of 0.29 mm.
  • the other frame has an internal dimension of 5 x 5 cm and a height of 0.38 mm.
  • the loaded pressing tool is placed in a hot press and a heating surface temperature of 170 ° C. is applied for 60 seconds. At the end of the pressing time, a pressing force of at least 10 tons is achieved. After the mold has cooled, the workpiece is removed and punched to its final dimensions.
  • a pressure-stable electrolysis MEE is obtained which is tight in the edge area and which can be installed directly in a PEM water electrolyzer.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Fuel Cell (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)

Abstract

L'invention concerne des unités membrane-électrodes utilisées pour l'électrolyse de l'eau (« unités membrane-électrodes pour électrolyse » (MEE)), qui contiennent une membrane conductrice d'ions, avec face avant et face arrière, une première couche catalytique pour la face avant, un premier substrat de répartition de gaz sur la face avant, une seconde couche catalytique sur la face arrière et un second substrat de répartition de gaz sur la face arrière. Le premier substrat de répartition de gaz présente à cet effet une extension en nappe inférieure à celle de la membrane conductrice d'ions, alors que le second substrat de répartition de gaz présente sensiblement la même extension en nappe que celle de la membrane conductrice d'ions (« conception semi-extensive »). Les MEE présentent en outre une surface membranaire libre non protégée, qui induit de meilleures propriétés d'adhérence du matériau d'étanchéité. L'invention concerne un procédé de production des produits MEE. L'invention permet d'obtenir des unités membrane-électrodes stables à la pression, étanches aux gaz et économiques, qui s'utilisent dans des d'électrolyseurs d'eau à membrane électrolytique polymère, dans des cellules à combustible régénératrices ou dans d'autres dispositifs électrochimiques.
EP04741011A 2003-07-14 2004-07-14 Unite membrane-electrodes pour electrolyse de l'eau Expired - Lifetime EP1652258B1 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE10331836 2003-07-14
US10/699,158 US20050014056A1 (en) 2003-07-14 2003-10-30 Membrane electrode unit for electrochemical equipment
PCT/EP2004/007802 WO2005006480A2 (fr) 2003-07-14 2004-07-14 Unite membrane-electrodes pour electrolyse de l'eau

Publications (2)

Publication Number Publication Date
EP1652258A2 true EP1652258A2 (fr) 2006-05-03
EP1652258B1 EP1652258B1 (fr) 2010-09-15

Family

ID=34066320

Family Applications (2)

Application Number Title Priority Date Filing Date
EP04763216.1A Expired - Lifetime EP1654776B1 (fr) 2003-07-14 2004-07-14 Unité membrane-électrode pour des installation électrochmiques
EP04741011A Expired - Lifetime EP1652258B1 (fr) 2003-07-14 2004-07-14 Unite membrane-electrodes pour electrolyse de l'eau

Family Applications Before (1)

Application Number Title Priority Date Filing Date
EP04763216.1A Expired - Lifetime EP1654776B1 (fr) 2003-07-14 2004-07-14 Unité membrane-électrode pour des installation électrochmiques

Country Status (6)

Country Link
US (1) US8394551B2 (fr)
EP (2) EP1654776B1 (fr)
KR (2) KR20060090216A (fr)
CA (2) CA2532794A1 (fr)
NO (1) NO20060701L (fr)
WO (2) WO2005006473A2 (fr)

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CA2532794A1 (fr) 2005-01-20
KR20060034705A (ko) 2006-04-24
WO2005006480A3 (fr) 2006-04-20
CA2532945C (fr) 2013-01-29
EP1652258B1 (fr) 2010-09-15
US8394551B2 (en) 2013-03-12
CA2532945A1 (fr) 2005-01-20
NO20060701L (no) 2006-04-12
EP1654776B1 (fr) 2013-09-11
WO2005006473A8 (fr) 2006-06-22
WO2005006480A2 (fr) 2005-01-20
US20070215461A1 (en) 2007-09-20
WO2005006473A3 (fr) 2005-11-10
KR20060090216A (ko) 2006-08-10
EP1654776A2 (fr) 2006-05-10
WO2005006473A2 (fr) 2005-01-20
KR101146519B1 (ko) 2012-07-05

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